Three volatile organic compounds (VOCs), benzene, cyclohexane, and dichloromethane, were adsorbed onto activated carbon fiber cloth. 1H (magic-angle spinning (MAS) and pulsed field gradient (PFG)) NMR techniques were carried out, and the signals were analyzed in terms of peak surface areas and shifts. These techniques were shown to be very useful for determining (i) the intrinsic quantification of adsorbed molecules (VOCs and/or water) in the porosity of the materials (the adsorption capacities ranged from 0.2 to 4 mol·kg-1); (ii) the mechanisms of interactions between adsorbed organic molecules and the carbon walls (illustrations of positions of the molecule inside the pore volume are proposed; the proton-wall distance was less than 0.15 nm); and (iii) the diffusivities (surface diffusion coefficients (DS) were estimated at ≈4.10-12 m2·s-1 for cyclohexane, ≈1.10-11 m2·s-1 for benzene, and ≈4.10-11 m2·s-1 for dichloromethane).